Volume 17, Issue 12 e202301927
Research Article

Copper Vacancy and LSPR-Activated MXene Synergistically Enabling Selective Photoreduction CO2 to Acetate

Chen Liao

Chen Liao

International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Shaanxi, 710049 P. R. China

These authors contributed equally to this work.

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Hongwei Zhou

Hongwei Zhou

International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Shaanxi, 710049 P. R. China

These authors contributed equally to this work.

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Shunxin Zhang

Shunxin Zhang

International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Shaanxi, 710049 P. R. China

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Feng Wang

Feng Wang

International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Shaanxi, 710049 P. R. China

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Prof. Ya Liu

Corresponding Author

Prof. Ya Liu

International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Shaanxi, 710049 P. R. China

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Prof. Liejin Guo

Corresponding Author

Prof. Liejin Guo

International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Shaanxi, 710049 P. R. China

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First published: 09 February 2024

Graphical Abstract

A highly effective photocatalytic system (VCu−CuInS2/MXene) was developed for transforming CO2 into acetate under full spectrum irradiation. The incorporation of the LSPR effect and defect engineering leads to a highly selective system.

Abstract

Photocatalytic CO2 conversion towards C2+ fuels is a promising technology for simultaneously achieving carbon neutrality and alleviating the energy crisis. However, this strategy is inefficient due to the difficulty of both multi-electron transfer and C−C coupling during C2+ formation. In this work, CuInS2/MXene heterostructure with Cu vacancy is rationally designed by in situ hydrothermal synthesis. The VCu−CuInS2/MXene heterostructure has a suitable band structure and tight interface contact. Catalytic performances under different testing conditions, in situ spectroscopy, and COMSOL simulation reveal that LSPR-activated MXene promotes the formation of crucial intermediate CH2* and triggers the C−C coupling process under near-infrared light, as the key to acetate. Moreover, in situ XPS analysis, DFT calculations, and photoelectrochemical characterizations unveil that copper vacancy can promote charge transfer from CuInS2 to MXene and boost local electron aggregation on the MXene, further enhancing the photocatalytic efficiency and selectivity of C2 products. Contributing to the synergistic effect of copper vacancy and plasmonic MXene, VCu−CuInS2/MXene achieved excellent CO2RR activity with an acetate evolution rate of 250.0 μmol/h/g and a selectivity of 97.5 % under the full spectrum irradiation, which is 38.8 and 3.3 times higher than that of VCu−CuInS2 and CuInS2/MXene, respectively.

Conflict of interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.